Molecular understanding of sulphuric acid-amine particle nucleation in the atmosphere

Autor(en)

Joao Almeida, Siegfried Schobesberger, Andreas Kuerten, Ismael K. Ortega, Oona Kupiainen-Maatta, Arnaud P. Praplan, Alexey Adamov, Antonio Amorim, Federico Bianchi, Martin Breitenlechner, Andre David, Josef Dommen, Neil M. Donahue, Andrew Downard, Eimear Dunne, Jonathan Duplissy, Sebastian Ehrhart, Richard C. Flagan, Alessandro Franchin, Roberto Guida, Jani Hakala, Armin Hansel, Martin Heinritzi, Henning Henschel, Tuija Jokinen, Heikki Junninen, Maija Kajos, Juha Kangasluoma, Helmi Keskinen, Agnieszka Kupc, Theo Kurten, Alexander N. Kvashin, Ari Laaksonen, Katrianne Lehtipalo, Markus Leiminger, Johannes Leppa, Ville Loukonen, Vladimir Makhmutov, Serge Mathot, Matthew J. McGrath, Tuomo Nieminen, Tinja Olenius, Antti Onnela, Tuukka Petaja, Francesco Riccobono, Ilona Riipinen, Matti Rissanen, Linda Rondo, Taina Ruuskanen, Filipe D. Santos, Nina Sarnela, Simon Schallhart, Ralf Schnitzhofer, John H. Seinfeld, Mario Simon, Mikko Sipila, Yuri Stozhkov, Frank Stratmann, Antonio Tome, Jasmin Troestl, Georgios Tsagkogeorgas, Petri Vaattovaara, Yrjo Viisanen, Annele Virtanen, Aron Vrtala, Paul E. Wagner, Ernest Weingartner, Heike Wex, Christina Williamson, Daniela Wimmer, Penglin Ye, Taina Yli-Juuti, Kenneth S. Carslaw, Markku Kulmala, Joachim Curtius, Urs Baltensperger, Douglas R. Worsnop, Hanna Vehkamaki, Jasper Kirkby

Abstrakt

Nucleation of aerosol particles from trace atmospheric vapours is

thought to provide up to half of global cloud condensation nuclei¹.

Aerosols can cause a net cooling of climate by scattering sunlight and

by leading to smaller but more numerous cloud droplets, which makes

clouds brighter and extends their lifetimes².

Atmospheric aerosols derived from human activities are thought to have

compensated for a large fraction of the warming caused by greenhouse

gases².

However, despite its importance for climate, atmospheric nucleation is

poorly understood. Recently, it has been shown that sulphuric acid and

ammonia cannot explain particle formation rates observed in the lower

atmosphere³. It is thought that amines may enhance nucleation^{4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16},

but until now there has been no direct evidence for amine ternary

nucleation under atmospheric conditions. Here we use the CLOUD (Cosmics

Leaving OUtdoor Droplets) chamber at CERN and find that dimethylamine

above three parts per trillion by volume can enhance particle formation

rates more than 1,000-fold compared with ammonia, sufficient to account

for the particle formation rates observed in the atmosphere. Molecular

analysis of the clusters reveals that the faster nucleation is explained

by a base-stabilization mechanism involving acid–amine pairs, which

strongly decrease evaporation. The ion-induced contribution is generally

small, reflecting the high stability of sulphuric acid–dimethylamine

clusters and indicating that galactic cosmic rays exert only a small

influence on their formation, except at low overall formation rates. Our

experimental measurements are well reproduced by a dynamical model

based on quantum chemical calculations of binding energies of molecular

clusters, without any fitted parameters. These results show that, in

regions of the atmosphere near amine sources, both amines and sulphur

dioxide should be considered when assessing the impact of anthropogenic

activities on particle formation.

Organisation(en)

Aerosolphysik und Umweltphysik

Externe Organisation(en)

European Organization for Nuclear Research (CERN), Universität Zürich (UZH), Universidade Técnica de Lisboa, Universidade da Beira Interior, IONICON Analytik GmbH, Leopold-Franzens-Universität Innsbruck, Carnegie Mellon University, California Institute of Technology (Caltech), University of Leeds, University of Eastern Finland, University of Helsinki, Finnish Meteorological Institute, Kyoto University, Stockholm University, Leibniz-Institut für Troposphärenforschung, Aerodyne Res Inc, Johann Wolfgang Goethe-Universität Frankfurt am Main, Russian Academy of Sciences

Journal

Nature

Band

502

Seiten

359-363

Anzahl der Seiten

11

ISSN

0028-0836

DOI

https://doi.org/10.1038/nature12663

Publikationsdatum

10-2013

Peer-reviewed

Ja

ÖFOS 2012

105204 Klimatologie, 105206 Meteorologie, 105904 Umweltforschung

Schlagwörter

Sustainable Development Goals

SDG 13 – Maßnahmen zum Klimaschutz

Link zum Portal

https://ucrisportal.univie.ac.at/de/publications/8ff5f4e1-582b-4694-82f1-896d0b511b36